Production of middle distillate range hydrocarbons by light olefin upgrading

ABSTRACT

An oligomerization system is provided for upgrading lower olefins to distillate hydrocarbons, especially useful as high quality jet or diesel fuels. The olefinic feedstock is reacted over a shape selective acid zeolite, such as ZSM-5, to oligomerize feedstock olefins and further convert recycled hydrocarbons. Reactor effluent is fractionated to recover a light-middle distillate range product stream and to obtain gasoline and heavy hydrocarbon streams for recycle.

CROSS-REFERENCE TO RELATED APPLICATION

This is a division of copending application Ser. No. 935,374, filed onNov. 26, 1986, now U.S. Pat. No. 4,849,186, which is acontinuation-in-part of application Ser. No. 699,882, filed Feb. 8, 1985now U.S. Pat. No. 4,720,600 which is a continuation-in-part ofapplication Ser. No. 654,348, filed Sept. 25, 1984, now U.S. Pat. No.4,547,612 and a continuation-in-part of application Ser. No. 616,376,filed June 1, 1984, now U.S. Pat. No. 4,504,691.

FIELD OF THE INVENTION

This invention relates to a continuous technique for the manufacture ofdistillate range hydrocarbons, such as jet aircraft engine fuel orkerosene In particular, it provides a system for operating an olefinsconversion plant wherein a oligomerization catalyst, such as shapeselective medium pore crystalline zeolite of the ZSM-5 type, is employedfor upgrading olefinic feedstocks containing lower alkenes at elevatedtemperature and pressure.

BACKGROUND OF THE INVENTION

Recent work in the field of olefin upgrading has resulted in a catalyticprocess for converting lower olefins to heavier hydrocarbons. Particularinterest is shown in a technique wherein distillate range hydrocarbonscan be synthesized over ZSM-5 type catalysts at elevated temperature andpressure to provide a product having substantially linear molecularconformations due to the ellipsoidal shape selectivity of certain mediumpore catalysts.

Conversion of olefins to gasoline and/or distillate products isdisclosed in U.S. Pat. Nos. 3,960,978 and 4,021,502 (Givens, Plank andRosinski) wherein gaseous olefins in the range of ethylene to pentene,either alone or in admixture with paraffins are converted into anolefinic gasoline blending stock by contacting the olefins with acatalyst bed made up of a ZSM-5 type zeolite. In U.S. Pat. No. 4,227,992Garwood and Lee disclose the operating conditions for the Mobil Olefinto Gasoline/Distillate (MOGD) process for selective conversion of C₃ ⁺olefins to mainly aliphatic hydrocarbons. In a related manner, U.S. Pat.Nos. 4,150,062 and 4,211,640 (Garwood et al) disclose a process forconverting olefins to gasoline components.

In the process for catalytic conversion of olefins to heavierhydrocarbons by catalytic oligomerization using a medium pore shapeselective acid crystalline zeolite, such as ZSM-5 type catalyst, processconditions can be varied to favor the formation of hydrocarbons ofvarying molecular weight. At moderate temperature and relatively highpressure, the conversion conditions favor C₁₀ ⁺ aliphatic product. Lowerolefinic feedstocks containing C₂ -C₈ alkenes may be converted; however,the distillate mode conditions do not convert a major fraction ofethylene. A typical reactive feedstock consists essentially of C₃ -C₆mono-olefins, with varying amounts of nonreactive paraffins and the likebeing acceptable components.

It is a main object of this invention to provide a continuous systemdevised for upgrading olefins to valuable middle distillate fuelproduct. It is a further object to provide an operable olefinsoligomerization technique to maximize production of light and middledistillate product, such as high quality jet fuel having a boiling rangeof about 165° to 290° C. (330°-550° F.).

SUMMARY OF THE INVENTION

A continuous system has been devised for converting a feedstockcomprising lower olefins to form higher hydrocarbons, particularlydistillate product. This system includes means for producing heavyhydrocarbons comprising distillate range compounds having asubstantially linear molecular conformation comprising means forcontacting olefinic feedstock in a catalytic reaction zone underoligomerization conditions at moderate reaction temperature and highpressure favorable to formation of high molecular weight aliphatichydrocarbons with a shape selective medium pore acidic crystallinesilicate zeolite catalyst in a reaction zone maintained under lowseverity conditions to prevent excessive cracking; means for recoveringoligomerized hydrocarbon effluent containing middle distillate rangehydrocarbon product, higher boiling hydrocarbons and lower boilinghydrocarbons; means for fractionating the effluent to obtain adistillate range product fraction, a higher boiling liquid fraction, anda lower boiling liquid fraction; and means for recycling higher andlower boiling liquid streams comprising at least a major portion of thehigher and lower boiling liquid fractions for further reaction in thereaction zone.

This technique is particularly useful for producing middle distillatehydrocarbons comprising C₉ to C₁₆ aliphatic compounds having asubstantially linear molecular conformation. These and other objects andfeatures of the invention will be understood from the following detaileddescription and drawings.

THE DRAWINGS

FIG. 1 is a schematic representation of a fixed bed reactor system andproduct separation system, according to the present invention, showingprocess flow streams and unit operations;

FIG. 2 is a graphic plot showing product distribution for a series ofpropylene conversion runs at various pressures;

FIG. 3 is a graphic plot of propylene conversion over HZSM-5 atdifferent space velocities; and

FIG. 4 is a schematic process diagram of an alternative embodiment ofthe invention;

FIG. 5 is a graphic plot of product distribution by carbon number atvarious pressures; and

FIG. 6 is a process flow sheet for an alternative embodiment.

DESCRIPTION OF THE PREFERRED EMBODIMENTS

Recent developments in zeolite technology have provided a group ofmedium pore siliceous materials having similar pore geometry. Mostprominent among these intermediate pore size zeolites is ZSM-5, which isusually synthesized with Bronsted acid active sites by incorporating atetrahedrally coordinated metal, such as Al, Ga, or Fe, within thezeolytic framework. These medium pore zeolites are favored for acidcatalysis; however, the advantages of ZSM-5 structures may be utilizedby employing highly siliceous materials or cystalline metallosilicatehaving one or more tetrahedral species having varying degrees ofacidity. ZSM-5 crystalline structure is readily recognized by its X-raydiffraction pattern, which is described in U.S. Pat. No. 3,702,866(Argauer, et al.), incorporated by reference.

The oligomerization/polymerization catalysts preferred for use hereininclude the crystalline aluminosilicate zeolites having a silica toalumina molar ratio of at least 12, preferable about 20:1 to 100:1, aconstraint index of about 1 to 12 and acid cracking activity of about50-200. Representative of the ZSM-5 type zeolites are ZSM-5, ZSM-11,ZSM-12, ZSM-23, ZSM-35 and ZSM-38. ZSM-5 is disclosed and claimed inU.S. Pat. No. 3,702,886 and U.S. Pat. No. Re. 29,948; ZSM-11 isdisclosed and claimed in U.S. Pat. No. 3,709,979. Also, see U.S. Pat.No. 3,832,449 for ZSM-12; U.S. Pat. No. 4,076,842 for ZSM-23; U.S. Pat.No. 4,016,245 for ZSM-35 and U.S. Pat. No. 4,046,839 for ZSM-38. Thedisclosures of these patents are incorporated herein by reference. Asuitable shape selective medium pore catalyst of fixed bed is a standardH-ZSM-5 zeolite (silica:alumina ratio=70:1) with alumina binder in theform of cylindrical extrudates of about 1-5 mm. Unless otherwise statedin this description, the catalyst shall consist essentially of thisstandard ZSM-5, which has an acid cracking value (α-value) of about160-200. Other pentasil catalysts which may be used in one or morereactor stage include a variety of medium pore shape selective (5 to 9A) siliceous materials such as borosilicates, ferrosilicates, and/oraluminosilicates disclosed in U.S. Pat. Nos. 4,414,423, 4,417,086,4,417,087 and 4,417,088, incorporated herein by reference.

Shape-selective oligomerization, as it applies to the conversion of C₂-C₁₀ olefins over ZSM-5, is known to produce higher olefins up to C₃₀and higher. As reported by Garwood in Intrazeolite Chemistry 23, (Amer.Chem. Soc., 1983), reaction conditions favoring higher molecular weightproduct are low temperature (200°-260° C), high pressure (300 psig orgreater), and long contact time (0.5-1 WHSV). The reaction under theseconditions proceeds through the acid-catalyzed steps of (1)oligomerization, (2) isomerization-cracking to a mixture of intermediatecarbon number olefins, and (3) interpolymerization to give a continuousboiling product containing all carbon numbers. The channel systems ofZSM-5 type catalysts impose shape-selective constraints on theconfiguration of the large molecules, accounting for the differenceswith other catalysts.

The following model reaction path for propylene is set forth forpurposes of explanation, and it should be taken as a theoretical path,as the process is presently understood by workers in the field. ##STR1##The desired oligomerization-polymerization products are C₁₀ ⁺substantially linear aliphatic hydrocarbons. As a result of having bothforward (polymerization) and reverse (cracking), a continuous molecularweight distribution will occur in the product which can be independentof the carbon number of the starting olefin. For example, Garwood haspreviously shown, at constant temperature and pressure, virtuallyidentical product distribution for feedstocks of ethylene (C₂ ⁼),propylene (C₃ ⁼), pentene (C₅ ⁼), hexene (C₆ ⁼)and decene C₁₀ ⁼.Structurally the final product is influenced by the pore structure ofthe catalyst. For low carbon number products (i.e., C₄, C₅) isomerdistribution is approximately at equilibrium. For the higher carbonnumbers, the structure is primarily a methyl-branched straight olefinicchain, with the maximum cross section of the chain limited by the5.4×5.6 Angstrom dimension of the largest ZSM-5 pore. At conditionschosen to maximize distillate range products (C₁₀ ⁺) the raw aliphaticproduct is essentially mono-olefinic with 10% or less of the double bondin the alpha position. Overall branching is not extensive, with mostbranches being methyl at about one branch per four/five carbon atoms.

The flowsheet diagram of FIG. 1 shows the process relationships of theinventive process, depicting the conversion of the C₃ -C₆ rich olefinicintermediate, multi-stage phase separation and recycle. Middledistillate hydrocarbons are recovered by fractionation and may be sentto a conventional hydrotreating unit for product finishing.

GENERAL PROCESS DESCRIPTION

The olefinic feedstock supply 1 is normally liquid and can be brought toprocess pressure by means of pump 10 and preheated by passingsequentially through a series of heat exchange means 11, 12 and reactanteffluent exchangers 14C, 14B, 14A and furnace 16 prior to entering thecatalytic reactor system 20.

A typical distillate mode first stage reactor system 20 is shown. Amulti-reactor system is employed with inter-zone cooling, whereby thereaction exotherm can be carefully controlled to prevent excessivetemperature above the normal moderate range of about 200° to 290° C.(400°-550° F.), especially in the final reaction zone While processpressure may be maintained over a wide range, usually from about 2800 toover 20,000 kPa (400-3000 psia), the preferred pressure is about 4000 to10,000 kPa (600 to 1500 psia). The feedstock is heated to reactiontemperature and carried sequentially through a series of zeolite beds20A, B, C wherein at least a portion of the olefin content is convertedto heavier distillate constituents. Advantageously, the maximumtemperature differential across only one reactor is about 30° C. (T=50°F.) and the space velocity (LHSV based on olefin feed) is about 0.1 to2, preferably about 1.0. The heat exchangers 14A and 14B provideinter-reactor cooling.

In a typical continuous process run under steady state conditions usinga standard HZSM-5 catalyst, the average reactor temperature in theseries of adiabatic fixed bed reactors is maintained below about 315° C.(600° F). In order to optimize formation of high molecular weight C₉ ⁺hydrocarbons, effluent temperature from the terminal reactor 20C is keptsubstantially below about 290° C. (550° F). Catalyst in the terminalposition is preferably the most active in the series, being fresh orregenerated to maintain a high alpha value. By controlling the moderatereaction temperature in the last two beds, undesired cracking of theproduct C₉ ⁺ hydrocarbons is minimized.

The reactor effluent is cooled in exchanges 12 and 14C beforefractionation. The effluent fractionation system has two main functions:(1) to provide primary means for separating suitable recycle materialsand (2) to provide secondary means for recovering refined productstreams of acceptable quality. The primary section is not required toprovide streams of clearly defined boiling point components; and,therefore, phase separator in combination with flashing and heatexchange equipment can provide adequate recycle economically. However,the secondary fractionation function requires distinct separationaccording to molecular weight and boiling point, which usually dictatesat least one distillation tower. While the embodiments disclosed hereininclude operatively connected separators, product splitters,debutanizers, etc., it is within the skill of the art to apply theinventive concept to a variety of effluent separation systems, toprovide the required recycle and product streams for a continuous lightolefin upgrading system according to the present invention.

The effluent mixture under process pressure or flashed enters a hightemperature separator (HTS) 26, wherein higher boiling product isrecovered as a liquid rich in C₁₆ ⁺ hydrocarbons; while vaporizingvolatile components of the effluent stream, including the light andintermediate hydrocarbons, such as C₁ to C₁₆ aliphatics. Preferably, themajor portion (e.g. 50% to more than 90 wt %) of C₁₆ hydrocarboncomponents are contained in the high boiling liquid fraction. Overheadvapor is withdrawn through conduit 27, cooled indirectly by incomingfeedstock in exchanger 11 to condense a major amount gasoline rangehydrocarbons for recovery in the second phase separation unit 30. Thiscondensed stream is withdrawn through conduit 32 for recycle andpressurized by pump means 34 prior to combining with feedstock inconduit 36. Advantageously, the major portion of C₅ to C₈ hydrocarboncomponents boiling below about 165° C. are contained in the liquifiedlower boiling recycle stream.

Liquid hydrocarbons rich in middle and heavy distillate are recoveredfrom the primary separation zone 26 at process pressure, preferablyabout 1000 to 1500 kPa (150 to 220 psia) and passed to product splittertower 50 for secondary fractionation to provide a middle distillateproduct fraction rich in C₉ -C₁₆ olefins and a C₁₆ ⁺ heavy distillatestream for recycle or recovery. A vapor overhead stream from the secondseparation zone 30 is sent directly through conduit 31 to thedistillation tower 60 to provide a middle distillate bottoms stream.Gasoline rich overhead from tower 60 is further fractionated indebutanizer tower 70, which provides C₅ -165° C. olefinic gasoline foradditional recycle or product along with C₃ -C₄ rich LPG.

Raw olefinic product may then be hydrotreated in a separate process step(not shown) to provide a paraffinic distillate product meeting jet fuelrequirements. Details of a mild hydrogenation treatment may be obtainedfrom U.S. Pat. No. 4,211,640, incorporated by reference, typically usingCo or Ni with W/Mo and/or noble metals. The hydrotreated stream may befurther fractionated for flash point stabilization.

There are several advantages to the process design. The lower boilingrange hydrocarbon recycle consists essentially of C₅ -C₈ hydrocarbons,with minor amounts of C₄ ⁻ components. This recycle material preferablyincludes at least b 50% of the C₅ to C₈ hydrocarbons from the reactoreffluent. Having a relatively high heat capacity, it provides a goodheat sink without diminishing feedstock olefin partial pressure andthereby maintains a high olefin partial pressure at reactor inlet. Theliquid recycle is economically repressurized by pumping, which requiresmodest power consumption.

Typical distillate mode oligomerization operations are conducted over afixed bed of HZSM-5/alumina extrudate catalyst using the techniquesdescribed in U.S. Pat. No. 4,456,779 (Owen et al.), U.S. Pat. No.4,433,185 (Tabak), and U.S. patent application Ser. No. 654,348 (filed25 Sept. 1984), incorporated herein by reference. Reactor sequencing andcatalyst regeneration are known in the art.

In order to demonstrate the effect of pressure on the process, propyleneis reacted at 204° C. and 0.4 WHSV over HZSM-5 in an isothermal reactionzone. FIG. 2 shows a correlation between boiling range of liquid productfrom 2400 to 10,400 kPa, with a low pressure run (274° C.) plotted forcomparison. Propylene conversion is essentially complete at 204° C.under these conditions, and the liquid product includes all carbonnumbers from C₆ to about C₃₆.

In FIG. 3, the effect of contact time is depicted by comparing two runsusing propylene feed at 204° C. and 3600 kPa. The liquid boilingplateaus in the higher space velocity run (2.7 WHSV) show evidence ofoligomers, corresponding to the trimer, tetramer and pentamer ofpropylene formed at 67% conversion during short residence. Thiscontrasts with the relatively smooth curve of a longer contact time (0.4WHSV). The preferred operation with space velocity less than 1 providesessentially complete conversion of C₃ -C₁₀ feedstock. It is acharacteristic of the reaction path that the liquid product boilingpoint curve for propylene is substantially similar to that of a C₁₀(1-decene) feed, at low space velocity (0.1 to 0.5), 277° C. (530° F.)reaction temperature. This suggests that the two widely different chargeolefins undergo a common intermediate stage.

An alternate embodiment of the inventive process is depicted in FIG. 4,which is a flow sheet for a continuous olefins upgrading plant employinga fixed bed catalytic reactor. Simplified effluent fractionation andrecycle streams are shown schematically, with reactor transfer and otherdetails being omitted. Referring to FIG. 4, fresh olefinic feed 101 ispressurized and preheated via exchangers 111, 112. The fresh lowerolefin feed may be fed directly to the primary reactor 120A combinedwith recycle 136 and heated in furnace 116 to reaction temperature.Optionally, the feedstock may be diverted around reactor 120A toposition B. The feedstock is passed over standard ZSM-5 catalyst in aseries of continuous downflow vertical fixed bed reactors 120. Theaverage reactor temperature is incrementally decreased from about 315°C. (600° F.) to 260° C. (500° F.), or higher, thereby favoring crackingin the first reactor A and oligomerization in the last reactor C. Aseries of high, middle and low temperature phase separators 127, 128,130 are employed to recover a high boiling liquid recycle stream 129 anda middle distillate-rich liquid product stream 128A, which is passed todistillation tower 150 for splitting into heavy distillate (290° C.⁺)and light distillate streams. The light distillate may be furthertreated by hydrogenation and flash point stabilization in a knownmanner. Gasoline and LPG are recovered by fractionating the overheadvapor from the low temperature separator, from which another recyclestream 130A is taken, which stream is rich in C₅ to C₈ hydrocarbons.Optionally the light hydrocarbon recycle from low temperature separator130 may be sent to the low temperature reactor(s) via conduit 130Btogether with diverted feedstock olefins, bypassing the highertemperature first reactor A and thereby avoiding substantial cracking.

In the following examples the average reactor temperature is maintainedwithin the range of 205° to 290° C. (400° to 550° F.), and a spacevelocity (WHSV based on feed olefin) of about 0.6 to 1.0. Threedifferent operating pressures are employed in successive continuous runsat about 4200 kPa (600 psig), 5600 kPa (800 psig) and at 10400 kPa (1500psig). Under these conditions, a feedstock consisting of 10.7 weightpercent propane, 27 wt % propylene, 26.2 wt % isobutane and 36.1 wt %butylene is converted.

In FIG. 5, the results of the three runs are plotted to show the productdistribution in the reactor effluent, employing gasoline recycle.Optimum jet fuel distillate hydrocarbons are produced in the C₉ to C₁₆range, corresponding to a normal boiling point of about 165° C. to 290°C. When the higher boiling 290°⁺ C. hydrocarbons are reprocessed underthe same reaction conditions a single pass conversion run yields anaverage increase of about 23 wt. % to light distillate (165°-290° C.)and 8 wt. % C₅ -165° C. gasoline range components in the effluent. Theproduct distribution of reprocessed 290°⁺ C. hydrocarbons is shown inTable I.

                  TABLE I                                                         ______________________________________                                        Yield from Reprocessed Heavy Distillate, 290°.sup.+ C.                 (550° F..sup.+)                                                                       DAYS ON STREAM                                                                6     7       8       9                                        ______________________________________                                        OPERATING CONDITIONS                                                          AVE. REAC. TEMP., F.                                                                           500     520     541   561                                    REAC. PRESS., PSIG                                                                             600     600     600   600                                    LHSV, (TOTAL)    1.00    1.00    1.00  1.00                                   WHSV, (TOTAL)    1.35    1.35    1.35  1.35                                   PRODUCT                                                                       DISTRIBUTION (WT %)                                                           C4               0.61    0.89    1.27  1.63                                   C5+-330 F.       6.74    7.72    7.40  9.17                                   330 F.-550 F.    24.90   23.84   22.83 21.80                                  550 F.+          67.74   67.55   68.50 67.40                                  ______________________________________                                    

Typical product specifications for jet fuels are given below.

                  TABLE II                                                        ______________________________________                                        Jet Fuel Volatility Specifications                                                     JP4    JP5       JP7                                                          (MIL-T-                                                                              (MIL-T-   (MIL-T-                                                      5624L) 5624L)    38219)    JET A                                     ______________________________________                                        10% BP     NS       401 (max) 385 (min)                                                                             400                                     (D86), °F.                     (max)                                   90% BP (D86),                                                                            473      NS        500     NS                                      °F. (max)                                                              End Point (D86),                                                                         518      554       550     572                                     °F. (max)                                                              Flash Point,                                                                             NS       140       140     100                                     °F. (min)                                                              ______________________________________                                    

A continuous system for upgrading lower olefin feedstock to higherhydrocarbons is depicted in FIG. 6, wherein ordinal numbers correspondwith elements in FIG. 1. Reactor means 220A, B, C is provided forcontacting the feedstock, via conduit 201, exchangers 211, 214A and B,with a shape selective medium pore acid zeolite catalyst under reactionconditions at elevated temperature in a pressurized reactor system 220comprising a series of catalytic reactor beds A, B, C to convertolefins. The heat exchangers 214 A, B provide means for incrementallydecreasing reactor temperature from a first reactor bed 220A in theseries to terminal reactor bed 220C to promote oligomerization in thelast reactor bed. First HTS separation means 226 separates reactoreffluent to separate volatile light and middle distillate hydrocarboncomponents into a first vapor phase stream and recovers heavy liquid forcatalytic cracking in reactor unit 220D, maintained at a temperature ofat least about 400° C. under conversion conditions to degrade the heavyhydrocarbons for recycle of cracked components via separator 230. Theheavy liquid stream contains at least 50% of those C₁₆ ⁺ hydrocarbonsrecovered in the reactor effluent.

Second LTS separation means 230 condenses a portion of the first vaporphase stream to recover a dominant portion of a light olefinic C6-C8stream. This can be recycle via distillation towers 250, 260 for furtherreaction in one or more serial reactor beds to promote oligomerization.The light recycle stream comprises a major portion of C₆ to C₈hydrocarbons recovered in the reactor effluent. Fractionation towers 250and 260 provide means for distilling the intermediate liquid productstream recovered from the second separation means to obtain a middledistillate product stream(eg-jet fuel) consisting essentially ofsubstantially linear C₉ -C₁₆ aliphatic hydrocarbons, along with minoramounts of LPG, gasoline and heavy diesel fuels, for instance.

The reactor system depicted contains multiple downflow adiabaticcatalytic zones in each reactor zone. The liquid hourly space velocity(based on total fresh feedstock) is about 1 LHSV. In the preferreddistillate mode the inlet pressure to the first oligomerization reactoris about 4200 kPa (600 psig total), with an olefin partial pressure ofat least about 1200 kPa. Based on olefin conversion of 50% of ethene,95% for propene, 85% for butene-1 and 75% for pentene-1, and exothermicheat of reaction is estimated at 450 BTU per pound of olefins converted.When released uniformly over the reactor beds, a maximum T in eachreactor is about 30° C.

Preferably the ZSM-5 catalyst is kept on stream until the coke contentincreases from 0% at the start of cycle (SOC) until it reaches a maximumof 30 weight % at the end of cycle (EOC) at which time it is regeneratedby oxidation of the coke deposits. Typically, a minimum 30 day totalcycle can be expected between regenerations. The reaction operatingtemperature depends upon its serial position. The system is operatedadvantageously in increasing the operating temperature of the firstreaction (Position A) from about 230°-255° C. (SOC) to about 270°C.-295° C. (EOC) at a catalyst aging rate of 3°-6° C./day. Reactors inthe second and subsequent Positions (B, C, etc) are operated at the sameSOC temperature; however, the lower aging rate (e.g. -3° C./day) incontinuous operation yields a lower EOC maximum temperature (e.g.--about275° C.) after about 7 days on stream. The end of cycle is signalledwhen the outlet temperature of the reactor in Position A reaches itsallowable maximum. At this time the inlet temperature is reduced tostart of cycle levels in order to avoid excessive coking over thefreshly regenerated catalyst when a reactor containing active catalystis brought on-line, after having been brought up to reaction pressurewith an effluent slip stream.

Partially deactivated catalyst from Position A is useful for cracking athigher temperatures (e.g. -400° C. to 600° C.) in Position D prior tocyclic regeneration. Regeneration of coked catalyst in situ may beeffected by a procedure described in U.S. Pat. No. 4,456,779 (Owen etal) and U.S. Pat. No. 4,560,536 (Tabak). A programmable logic controllermay be employed to control the sequencing of valve operations during allstages of reactor system operation. When regeneration is completed, thereactor is blocked off from the regeneration loop and brought up toreaction pressure with a slip stream from the process reactor effluentline. To reconnect the regenerated reactor in the proper serial positionwhen full flow is established in the regenerated reactor in Position C,reactor C is paralleled with preceding reactor B, receiving flow fromthe first reactor A, etc. The partially deactivated catalyst bed istransferred from Position A to cracking operation in Position D. Finallythe fully coked catalyst bed is blocked in, depressured, and repressuredwith nitrogen, then opened to the regeneration circuit. Thus eachreactor will move from Position C to Position B to Position A toPosition D before being taken off-line for catalyst regeneration.

Various modifications can be made to the system, especially in thechoice of equipment and non-critical processing steps. While theinvention has been described by specific examples, there is no intent tolimit the inventive concept as set forth in the following claims.

What is claimed is:
 1. In a continuous system for upgrading lower olefinfeedstock to higher hydrocarbons including means for combining olefinicfeedstock with a pressurized liquid diluent stream comprising C₅ ⁺olefins, reactor means for contacting the diluted feedstock with a shapeselective medium pore acid zeolite catalyst under reaction conditions atmoderate temperature in a pressurized reactor system comprising a seriesof catalytic reactor beds to convert olefins and recover reactoreffluent at reaction conditions; the improvement which comprises:meansfor incrementally decreasing reactor temperature from a first reactorbed in the series to a last reactor bed to promote oligomerization inthe last reactor bed; and first separation means operatively connectedto receiver effluent from said last reactor bed for separating reactoreffluent in a primary phase separation zone to vaporize light and middledistillate hydrocarbon components into a first vapor phase stream andrecover from the primary separation zone a heavy liquid hydrocarbonrecycle stream, said heavy liquid stream containing at least 50% ofthose C₁₆ ⁺ hydrocarbons recovered in the reactor effluent; recyclemeans for passing the heavy liquid hydrocarbon recycle stream from saidfirst separation means to said first reactor bed, maintained underconditions to degrade heavy hydrocarbons; second separation meansoperatively connected to receive said first vapor phase stream forcondensing a light portion of the first vapor phase and recovering adominant portion of a light olefinic recycle stream as an intermediateliquid product stream for further reaction in a lower temperature serialreactor bed in said series of reactor beds to promote oligomerization,said light recycle stream comprising a major portion of C₆ to C₈hydrocarbons recovered in the reactor effluent; and fractionation meansfor distilling the intermediate liquid product stream recovered from thesecond separation means to obtain a distillate product stream consistingessentially of substantially linear C₉ -C₁₆ aliphatic hydrocarbons.
 2. Acontinuous system for upgrading lower olefin feedstock to higherhydrocarbons comprisingreactor means for contacting the feedstock with ashape selective medium pore acid zeolite catalyst under reactionconditions at elevated temperature in a pressurized reactor systemcomprising a series of catalytic reactor beds to convert olefins andrecover reactor effluent at reaction conditions; the improvement whichcomprises: means for incrementally decreasing reactor temperature from afirst reactor bed in the series to a last reactor bed to promoteoligomerization in the last reactor bed; and first separation meansoperatively connected to receive effluent from said last reactor bed forseparating reactor effluent to vaporize light and middle distillatehydrocarbon components into a first vapor phase stream and recover aheavy liquid hydrocarbon recycle stream, said heavy liquid streamcontaining at least 50% of those C₁₆ ⁺ hydrocarbons recovered in thereactor effluent; recycle means for passing the heavy liquid hydrocarbonrecycle stream from said first separation means to said first reactorbed, maintained under conditions to degrade heavy hydrocarbons; secondseparation means operatively connected to receive said first vapor phasestream for condensing a light portion of the first vapor phase andrecovering a dominant portion of a light olefinic vapor as anintermediate liquid product stream recycle stream for further reactionin a lower temperature serial reactor bed in said series of reactor bedsto promote oligomerization, said light recycle stream comprising a majorportion of C₆ to C₈ hydrocarbons recovered in the reactor effluent; andfractionation means for distilling the intermediate liquid productstream recovered from the second separation means to obtain a distillateproduct stream consisting essentially of substantially linear C₉ -C₁₆aliphatic hydrocarbons.
 3. A cyclic reactor system for catalyticupgrading of olefinic hydrocarbon feedstock in a serially connectedmultiple catalyst zone reactor system comprising fixed catalyst bedpressurized reactors each having a porous bed zone of conversioncatalyst particles, which comprises:first stage plural serial reactormeans for contacting the feedstock in a first catalyst zone atmoderately elevated temperature under conditions favorable forconversion of a first reactor stream; means for separating a first stageeffluent stream into a light olefinic hydrocarbon recycle stream, at C₉-C₁₆ product stream and a second heavier hydrocarbon stream containingC₁₆ ⁺ hydrocarbons; fluid handling means for recycling at least aportion of the light olefinic hydrocarbon stream to an intermediatereactor in said first stage reactor means; fixed bed cracking reactormeans containing a porous bed of partially deactivated conversioncatalyst particles for contacting the heavier hydrocarbon stream fromthe first stage separation means at elevated cracking temperature underconditions favorable for conversion of the heavier hydrocarbons; cyclicfluid handling means for connecting the first stage serial reactors inoperative fluid flow relationship whereby fresh or regenerated catalystin a first stage terminal reactor position receives effluent from atleast one preceding first stage reactor operating at moderately elevatedoligomerization temperature, said preceding first stage reactorcontaining catalyst of less activity than said catalyst in the firststage terminal reactor; fluid handling means for sequencing reactorsystem effluent flow to reconnect a preceding first stage reactor inposition of said cracking reactor to receive the heavier hydrocarbonstream; means for increasing temperature in said previously precedingfirst stage reactor to cracking temperature conditions; means forremoving an inactivated catalyst reactor from preceding reactor fromcracking reactor conversion service and connecting said inactivatedcatalyst reactor in fluid flow relationship with a catalyst regenerationloop for catalyst reactivation; means for advancing the terminal reactorin the first stage to a preceding serial position in the first stage;and said fluid handling means including means for adding a fresh orregenerated catalyst reactor in the first stage terminal position.
 4. Acontinuous system for producing heavy hydrocarbons comprising distillaterange compounds having a substantially linear molecular conformationfrom lower olefins, comprisingmulti-zone plural reactor means forcontacting olefinic feedstock in a series of catalytic reaction zoneswith a shape-selective medium pore acidic crystalline silicate zeolitecatalyst under low severity conditions to prevent excessive cracking;heating and pressure means for maintaining in the reaction zoneoligomerization conditions of moderate temperature and high pressurefavorable to formation of high molecular weight aliphatic hydrocarbons;separation means comprising primary and secondary phase separation meansfor recovering oligomerized hydrocarbon effluent containing middledistillate range hydrocarbons, high boiling hydrocarbons and lowerboiling hydrocarbons; means for fractionating the effluent to obtain adistillate range product fraction, a high boiling range liquid fractionand a lower boiling liquid fraction; fluid handling means for recyclingat least a portion of lower boiling liquid fraction to an intermediatereactor zone in the multi-zone reactor means for further conversiontherein; and fluid handling means for recycling at least a major portionof the higher boiling liquid fraction for further reactor in a primaryreaction zone of said multi-zone reactor means.
 5. The system of claim 4wherein the multi-zone reactor system comprises a series of primary,intermediate and terminal operatively connected fixed bed adiabaticcatalytic reactors, with inter-reactor cooling, and including means forpassing recycled heavy liquid hydrocarbon through substantially all ofthe multi-zone reactor system.
 6. The system of claim 4 wherein thecrystalline silicate zeolite catalyst comprises aluminosilicate havingthe structure of HZSM-5.